胶凝剂对Cu/Zn/Al浆状催化剂一步法合成气催化制乙醇的影响  

Effect of gelling agent on Cu/Zn/Al slurry catalysts prepared by complete liquid-phase for one-step ethanol synthesis

作　　者：芦潇 张琳[1] 刘雷强 黄伟[1] 

机构地区：[1]太原理工大学煤科学与技术教育部与山西省共建重点实验室,山西太原030024

出　　处：《天然气化工—C1化学与化工》2017年第6期21-28,共8页Natural Gas Chemical Industry

基　　金：国家自然科学基金重点项目(21336006)

摘　　要：采用完全液相法制备了Cu-Zn-Al催化剂,不添加任何助剂,在醇解法的基础上,分别加入了作为胶凝剂的硝酸、柠檬酸溶液并排除了蒸馏水的影响制备了不同结构的前躯体,在浆态床反应器中考察了其催化CO加氢合成乙醇的反应性能,通过XRD、N_2吸附、H_2-TPR、NH_3-TPD和TEM等方法对催化剂进行了表征分析。结果表明:添加柠檬酸所制备的催化剂中存在与Zn、Al组分相互作用较强的高温难还原铜物种,铜晶粒尺寸、比表面积、以及弱酸量与强酸量的比率较大,孔径结构稳定。其CO转化率达37.7%,乙醇占总醇的质量分数可高达42.6%,在96h的催化剂活性评价期间内未见失活。The Cu-Zn-Al catalysts without other metal elements were prepared by the complete liquid-phase method. Based on the alcoholysis method, nitric acid and citric acid solutions were respectively added as gelling agent and the influence of distilled water was excluded to obtain the precursors with different structures. The catalysts were used for hydrogenation of CO in a slurry bed reactgr, and all of the fresh and used catalysts were characterized by XRD, N2-adsorption, H2-TPR, NH3-TPD and TEM. The results show that the using citric acid as gelling agent to prepare the catalyst can enhance interaction between the copper component and the Zn and Al components, increase the grain size of Cu, specific surface area and the ratio of weak acid and strong acid, and provide the catalyst a stable pore structure, which results in a high CO conversion of up to 37.7% and a high mass ratio of ethanol to total alcohols of up to 42.6% and the activity of catalyst can be maintained 96h.

关 键 词：铜基催化剂 完全液相法 凝胶剂 合成气 乙醇 浆态床 

分 类 号：O643.3[理学—物理化学] TQ426[理学—化学]